Highly dispersed Pt/Co3O4 catalyst constructed by vacancy defect inductive effect for enhanced catalytic propane total oxidation

doi:10.1016/S1872-2067(25)64736-X

Chinese Journal of Catalysis ›› 2025, Vol. 75: 21-33.DOI: 10.1016/S1872-2067(25)64736-X

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Highly dispersed Pt/Co₃O₄ catalyst constructed by vacancy defect inductive effect for enhanced catalytic propane total oxidation

Feng Chao^a^,^c^,^d^,^*(), Xiong Gaoyan^c, Chen Chong^c, Lin Yan^b^,^*(), Wang Zhong^d, Lu Yukun^c, Liu Fang^c, Li Xuebing^d, Liu Yunqi^c, Zhang Runduo^e^,^*(), Pan Yuan^c^,^*()

^aCollege of Chemical and Biological Engineering, Shandong University of Science and Technology, Qingdao 266590, Shandong, China
^bCollege of Energy Storage Technology, Shandong University of Science and Technology, Qingdao 266590, Shandong, China
^cState Key Laboratory of Heavy Oil Processing, College of Chemistry and Chemical Engineering, China University of Petroleum (East China), Qingdao 266580, Shandong, China
^dKey Laboratory of Biofuels, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao 266101, Shandong, China
^eState Key Laboratory of Chemical Resource Engineering, Beijing Key Laboratory of Energy Environmental Catalysis, Beijing University of Chemical Technology, Beijing 100029, China

Received:2025-03-10 Accepted:2025-05-10 Online:2025-08-18 Published:2025-07-22
Contact: *E-mail: fengchao@sdust.edu.cn (C. Feng),linyan09@sdust.edu.cn (Y. Lin),zhangrd@mail.buct.edu.cn (R. Zhang), panyuan@upc.edu.cn (Y. Pan).
Supported by:
Taishan Scholars Program of Shandong Province(tsqn201909065);National Natural Science Foundation of China(22108306);National Natural Science Foundation of China(21878334);National Natural Science Foundation of China(22478432);National Natural Science Foundation of China(22109090);National Natural Science Foundation of China(22178388);National Natural Science Foundation of China(22406191);Shandong Provincial Natural Science Foundation(ZR2024JQ004);Shandong Provincial Natural Science Foundation(ZR2021YQ15);Shandong Provincial Natural Science Foundation(ZR2023MB032);Qingdao New Energy Shandong Laboratory Open Project(QNESL OP202310);Qingdao Natural Science Foundation(23-2-1-14-zyyd-jch)

Abstract

Abstract:

Directional design of efficient catalysts for volatile organic compounds degradation remains a complex, yet effective and challenging process. Herein, oxygen-rich vacancy Co3O4-anchored Pt catalysts were prepared through atom-trapping strategy and relevant vacancy defect inductive effect was proposed. The 0.6Pt/VO-Co3O4 catalyst presented a reaction rate value of 32.2×10-5 mol·gcat-1·s-1 at 160 °C for catalytic propane total oxidation, which was nearly 5 times the reaction rate of Co3O4 (6.7×10-5 mol·gcat-1·s-1). Also, it exhibited excellent water-resistance and catalytic stability. The Pt atoms were stabilized on the Co3O4 surface by vacancy defects to improve dispersion. Meanwhile, the vacancy defect inductive effect induced stronger electron interaction between Pt and Co3O4 on the surface, thus promote the redox ability at low-temperature. The mobility and oxygen-activating ability of surface lattice oxygen were also strengthened by the vacancy defect inductive effect. This facilitated the generation of more surface-active oxygen species for the cleavage of C-H bond and the deep oxidation of intermediate species. Overall, this study proposed a novel concept the fabrication of highly efficient catalysts for the purpose of catalytic oxidation.

Key words: Propane total oxidation, Pt/Co₃O₄, Oxygen vacancy, Defect inductive effect, Synergetic catalysis

Feng Chao, Xiong Gaoyan, Chen Chong, Lin Yan, Wang Zhong, Lu Yukun, Liu Fang, Li Xuebing, Liu Yunqi, Zhang Runduo, Pan Yuan. Highly dispersed Pt/Co₃O₄ catalyst constructed by vacancy defect inductive effect for enhanced catalytic propane total oxidation[J]. Chinese Journal of Catalysis, 2025, 75: 21-33.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(25)64736-X

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Figures/Tables 8

Fig. 1. (a) Illustration of the synthesis of Pt/VO-Co3O4 catalysts. SEM (b), TEM (c), HRTEM (d), EDS-mapping (e) and HAADF-STEM (f) images of 0.6Pt/VO-Co3O4 catalysts.

Fig. 2. The Co XANES (a) and R-space FT EXAFS (b) of 0.6Pt/Co3O4 and 0.6Pt/VO-Co3O4 catalysts Co K-edge. Pt XANES (c) and R-space FT EXAFS (d) of 0.6Pt/Co3O4 and 0.6Pt/VO-Co3O4 catalysts Pt L-edge.

Fig. 3. EPR spectra (a), Raman spectra (b), bond calculated on the basis of Hooke’s law (c), Co 2p (d), O 1s (e) and Pt 4d (f) XPS spectra, O2-TPD (g), ESR spectrum (h) and H2-TPR spectra (i) of 0.6Pt/Co3O4 and 0.6Pt/VO-Co3O4 catalysts.

Fig. 4. Propane conversion in dry (a) and humid (b) atmosphere, stability in humid atmosphere (c) with 5 vol% H2O of 0.6Pt/Co3O4 and 0.6Pt/VO-Co3O4 catalysts. (d) Correlation between activities and surface species ratio.

Fig. 5. Dependence of reaction rate on partial pressure of propane of Pt/SiO2, Co3O4, VO-Co3O4 (a) and 0.6Pt/Co3O4, 0.6Pt/VO-Co3O4 (b), and oxygen of Pt/SiO2, Co3O4, VO-Co3O4 (c) and0.6Pt/Co3O4, 0.6Pt/VO-Co3O4 (d).

Table 1 Rate expressions of propane oxidation over Pt/Co3O4 and Pt/VO-Co3O4 catalysts.

Catalyst	Rate expression
Pt/SiO₂	r = 1.72 × 10^-4[C₃H₈]^1.01[O₂]^-0.57
Co₃O₄	r = 1.85 × 10^-4[C₃H₈]^1.01[O₂]^-0.86
V_O-Co₃O₄	r = 2.44 × 10^-4[C₃H₈]^1.00[O₂]^-0.84
0.3Pt/Co₃O₄	r = 3.42 × 10^-4[C₃H₈]^1.02[O₂]^-0.69
0.6Pt/Co₃O₄	r = 3.50 × 10^-4[C₃H₈]^0.99[O₂]^-0.70
1.2Pt/Co₃O₄	r = 3.43 × 10^-4[C₃H₈]^0.99[O₂]^-0.74
0.3Pt/V_O-Co₃O₄	r = 5.38 × 10^-4[C₃H₈]^0.99[O₂]^-0.70
0.6Pt/V_O-Co₃O₄	r = 5.99 × 10^-4[C₃H₈]^0.98[O₂]^-0.62
1.2Pt/V_O-Co₃O₄	r = 3.50 × 10^-4[C₃H₈]^1.00[O₂]^-0.75

Fig. 6. In-situ DRIFTs of propane oxidation over Co3O4 (a), VO-Co3O4 (b), 0.6Pt/Co3O4 (c) and 0.6Pt/VO-Co3O4 (d). In-situ DRIFTs signal difference between Co3O4 and VO-Co3O4 (e), 0.6Pt/Co3O4 and 0.6Pt/VO-Co3O4 (f).

Fig. 7. Charge density difference plot generated for Pt loading on the surface of Pt/VO-Co3O4 (a) and Pt/Co3O4 (b). The isosurface value is 0.005 e bohr-3. The yellow and blue represent positive and negative. (c) Pt PDOS. O dissociation energies (d), O2 adsorption AIMD (e), DOS (f) of C3H8 adsorbed on Co3O4, Pt/VO-Co3O4 and Pt/Co3O4. (g) Change of Gibbs free energy during propane initial oxidation of Co3O4, Pt/VO-Co3O4 and Pt/Co3O4. The models of IS and TS are shown in Supporting Information.

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Highly dispersed Pt/Co₃O₄ catalyst constructed by vacancy defect inductive effect for enhanced catalytic propane total oxidation

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